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In 1965, the Supermarionation TV series Stingray (1964 – 65), which followed the underwater adventures of Troy Tempest and the World Aquanaut Security Patrol (WASP), was given with its own comic. The first issue of TV Century 21 was published on 23 January 1965, capitalising on the popularity of the latest Gerry Anderson-produced TV series. In contrast with TV Comic, which was a traditional strip comic, TV Century 21 was conceived as a newspaper for children with a front page containing "Stop press"-style news items and photographs.

Although production on Supercar (1961 – 62) and Fireball XL5 (1962 – 63) had ended prior to the launch of TV Century 21, they were still being broadcast sporadically on ATV in the United Kingdom, and therefore also appeared in the comic. Thunderbirds (1965 – 66) was not featured until issue 52, but one of the series' main characters, the aristocratic Lady Penelope Creighton-Ward, appeared from issue 1. Fireball XL5, Stingray and Lady Penelope were the first three colour strips whose origins can be traced to the first issue. The front covers were also in colour, with photographs from one or more of the Anderson series or occasionally of the stars of the back page feature.

TV21 also extended its licensing beyond the Anderson productions, and for its first two years published strip adventures based on extraterrestrial Doctor Who villains the Daleks, the early scripts for which had the approval of Dalek creator Terry Nation.

The comic dropped the "Century" from its title in January 1968, after 155 issues, and became known as TV21. The previous year, the character of the "indestructible" Captain Scarlet, the hero of Captain Scarlet and the Mysterons (1967 – 68), had made his first appearance. The backstory of the Mysterons, Scarlet's Martian enemies, was being revealed in TV Tornado, another City Magazines publication. In September 1968, after 192 issues, TV21 merged with TV Tornado to form TV21 and Tornado.

The majority of the strips in TV Century 21 were set in the same shared future history. Even strips without a related TV series tied into it; for example, Special Agent 21 was set in the relative "past" and depicted the formation of the World Space Patrol seen in Fireball XL5.[3] The primary setting was the 2060s, with each newspaper-style issue covering the "top stories" of the decade. Earth was depicting as having a World Government — based in the fictional Unity City, Bermuda and incorporating a President and a Senate — whose authority encompassed most of the planet. Besides Spectrum, the World Navy, the World Aquanaut Security Patrol (WASP) and the World Space Patrol, all of which were seen in the Anderson series, the future Earth also boasted a World Army, World Air Force and Universal Secret Service (USS).

Elements of these would feature in multiple strips, including ones based on other series; elements of Fireball XL5 appeared several times in the Captain Scarlet adventures. Various textual commentaries established backstories for the characters that also connected the various series; for example, some of the Spectrum officers seen in Captain Scarlet were revealed to be former World Space Patrol agents. This did not necessarily contradict any of the TV series themselves as all were assumed to be set in the mid-21st century at least up until Captain Scarlet; Anderson's final two Supermarionation series, Joe 90 (1968 – 69) and The Secret Service (1969), had more contemporary settings.

A recurring plot element was the fictional Eastern European nation of Bereznik, a country not part of and hostile to the World Government. It appeared most frequently in the Thunderbirds and Lady Penelope strips, usually as an antagonist.[4]

On 18 January 1969, Anderson's latest Supermarionation production, Joe 90, made the transition from TV series to comic. This publication did not endure, however, merging with TV21 and Tornado in September 1969 after only 34 issues. At this time, the issue numbering of TV21 and Joe 90, as the comic was now called, was reset to 1, with a "New Series No." printed on the front cover. While the general format of the old comic was preserved, the Thunderbirds and Joe 90 strips were now printed in black and white in favour of the new colour favourites Star Trek (1966 – 69) and Land of the Giants (1968 – 70). The Joe 90 aspect gradually disappeared from the comic, whose name reverted to TV21 after 36 issues (the 278th overall). TV21 ceased publication in 1971 following its merger with Valiant.

In the UK, a sister publication was launched in the form of Lady Penelope, which featured Frank Langford's Lady Penelope comic strip. The comic ran for 204 issues; after 123 issues, the title was shortened to Penelope. It also included an Angels series of adventures as a prelude to the TV debut of Captain Scarlet and the Mysterons.